Plasma-Catalysis of Nonoxidative Methane Coupling: A Dynamic Investigation of Plasma and Surface Microkinetics over Ni(111).
Plasma-Catalysis of Nonoxidative Methane Coupling: A Dynamic Investigation of Plasma and Surface Microkinetics over Ni(111).
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DOI：
10.1021/acs.jpcc.2c03503
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发表时间：
2022-12-01
影响因子：
3.7
通讯作者：
Kechagiopoulos, Panagiotis N.
中科院分区：
文献类型：
--
作者：
Maitre, Pierre-Andre;Bieniek, Matthew S.;Kechagiopoulos, Panagiotis N.
在零维（0 D）等离子体模型中建立了一个非均相催化微动力学模型，用于研究Ni（111）催化剂上甲烷非氧化偶联反应的动力学过程，其停留时间和功率密度与实验反应器一致.微观动力学模型是热力学一致的，并基于Ni（111）表面物种的化学吸附热进行参数化。的表面网络明确占等离子体物种，即分子，自由基，和振动激发态，通过吸附和Eley-Rideal反应与催化剂活性位点的相互作用。Fridman-Macheret模型用于描述振动激发的CH 4，H2和C2 H6的解离吸附速率的增强。结合先前开发的详细的动力学方案的非热甲烷等离子体，0 D模拟结果带来的见解等离子体相和催化剂之间的复杂的动态相互作用在甲烷非氧化偶联。差分营业额频率实现等离子体催化高于那些等效的等离子体和催化模拟相结合，但是，这种性能只能暂时维持。通过等离子体内的电子碰撞从乙烷脱氢产生的氢被发现快速饱和表面，甚至促进表面CH 3 * 转化回甲烷。
A heterogeneous catalytic microkinetic model is developed and implemented in a zero-dimensional (0D) plasma model for the dynamic study of methane nonoxidative coupling over Ni(111) at residence times and power densities consistent with experimental reactors. The microkinetic model is thermodynamically consistent and is parameterized based on the heats of chemisorption of surface species on Ni(111). The surface network explicitly accounts for the interactions of plasma species, namely, molecules, radicals, and vibrationally excited states, with the catalyst active sites via adsorption and Eley–Rideal reactions. The Fridman–Macheret model is used to describe the enhancement of the rate of the dissociative adsorption of vibrationally excited CH4, H2, and C2H6. In combination with a previously developed detailed kinetic scheme for nonthermal methane plasma, 0D simulation results bring insights into the complex dynamic interactions between the plasma phase and the catalyst during methane nonoxidative coupling. Differential turnover frequencies achieved by plasma-catalysis are higher than those of equivalent plasma-only and catalysis-only simulations combined; however, this performance can only be sustained momentarily. Hydrogen produced from dehydrogenation of ethane via electron collisions within the plasma is found to quickly saturate the surface and even promote the conversion of surface CH3* back to methane.
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影响因子：
15.1
作者：
Andersen, J. A.;Christensen, J. M.;Jensen, A. D.
通讯作者：
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影响因子：
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